Mechanism of Methanol Decomposition over Single-Site Pt1/CeO2 Catalyst: A DRIFTS Study

Single-site catalysts have drawn broad attention in catalysis because of their maximum atomic utilization and unique catalytic performance. Early work in our group has shown a 40-fold higher activity of methanol decomposition over single-site Pt-1/CeO2 catalyst than CeO2 supported 2.5 nm Pt nanoparticles, while a molecular-level understanding of such enhancement is lacking. Herein, the reaction mechanism of methanol decomposition over Pt-1/CeO2 was carefully investigated using in situ DRIFTS, and a reaction pathway was proposed. Methanol molecules were dissociatively adsorbed on nanoceria support first, followed by the diffusion of as-formed methoxy species onto Pt single sites where the dehydrogenation occurs and results in the weakly bonded CO. The ease of methanol dissociative adsorption on nanoceria support and the tailored electronic property of Pt-1 via the metal-support interaction are believed to be strongly correlated with the high activity of Pt-1/CeO2.

Automated summary

Research has shown that the activity of Pt-1 / CeO2 catalyst surpasses that of CeO2 supported 2.5 nm Pt nanoparticles by 40-fold. The mechanism involves dissociative adsorption of methanol molecules on nanoceria support followed by diffusion onto Pt single sites for dehydrogenation, resulting in weakly bonded CO.